With an ever-increasing global population, the need for avant-garde sources of energy continues to advance as well. An alternative source of energy can be found via the implementation of artificial photosynthesis to produce hydrogen gas. Therefore, the development of more active and robust catalysts is necessary in order to make artificial photosynthesis a viable method of hydrogen generation. Recent studies have shown that metal complexes with redox non-innocent ligands and pendant base groups are highly active for proton reduction. Ni(EtPyPDI)2+ has shown to be a promising catalyst by producing hydrogen gas using Ru(bpy)32+and ascorbic acid generating turnover numbers of 1400. Because the activity of this catalyst is in part due to both the pKa and hemi-lability of the pendant base, substitution of this group may lead to improved activity. In this project, the pyridine rings were replaced with imidazole rings to synthesize Ni(EtImPDI)2+. The increased basicity of the ligands resulted in a less labile ligand and more electron rich metal ion, leading to lower catalytic activity. An in-depth computational analysis supported the experimental findings. Coordination and evaluation for the ligand with other common metals such as cobalt is also under investigation.

Investigation of Ni(EtImPDI)2+as a catalyst for light-driven hydrogen production

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